abstract

Highly selective removal of Cesium and Strontium is critical for waste treatment and environmental remediation. Cesium-137 is a beta-gamma emitter and Strontium-90 is a beta emitter with respective half-lives of 30 and 29 years. Both elements are present at many nuclear sites. Cesium and Strontium can be found in wastewaters at Washington State’s Hanford Site, as well as in wastestreams of many Magnox reactor sites. Cesium and Strontium are found in the Reactor Coolant System of light water reactors at nuclear power plants. Both elements are also found in spent nuclear fuel and in high-level waste (HLW) at DOE sites. Cesium and Strontium are further major contributors to the activity and the heat load. Therefore, technologies to extract Cesium and Strontium are critical for environmental remediation waste treatment and dose minimization. Radionuclides such as Cesium-137 and Strontium-90 are key drivers of liquid waste classification at light water reactors and within the DOE tank farm complexes. The treatment, storage, and disposal of these wastes represents a major cost for nuclear power plant operators, and comprises one of the most challenging technology-driven projects for the DOE Environmental Management (EM) program. Extraction technologies to remove Cesium and Strontium have been an active field of research. Four notable extraction technologies have been developed so far for HLW: solvent extraction, prussian blue, crystalline silicotitanate (CST) and organic ion-exchangers (e.g., resorcinol formaldehyde and SuperLig). The use of one technology over another depends on the specific application. For example, the waste treatment plant (WTP) at Hanford is planning on using a highly-selective organic ion-exchange resin to remove Cesium and Strontium. Such organic ion-exchangers use molecular recognition to selectively bind to Cesium and Strontium. However, these organic ion-exchangers are synthesized using multi-step organic synthesis. The associated cost to synthesize organic ion-exchangers is prohibitive and seriously limits the scope of applications for organic ion-exchangers. Further issues include resin swelling, potential hydrogen generation and precluding final disposal by vitrification without further issues. An alternative to these issues of organic ion-exchangers is emerging. Inorganic ion-exchangers offer a superior chemical, thermal and radiation stability which is simply not achievable with organic compounds. They can be used to remove both Cesium as well as Strontium with a high level of selectivity under a broad pH range. Inorganic ion-exchangers can operate at acidic pH where protons inhibit ion exchange in alternative technologies such as CST. They can also be used at high pH which is typically found in conditions present in many nuclear waste types. For example, inorganic ion-exchangers have shown significant Strontium uptake from pH 1.9 to 14. In contrast to organic ion-exchangers, inorganic ion-exchangers are not synthesized via complex multi-step organic synthesis. Therefore, inorganic ion-exchangers are substantially more cost-effective when compared to organic ion-exchangers as well as CST. Selective removal of specified isotopes through ion exchange is a common and proven treatment method for liquid waste, yet various aspects of existing technologies leave room for improvement with respect to both cost and effectiveness. We demonstrate a novel class of inorganic ion-exchangers for the selective removal of cesium and strontium (with future work planned for uranium removal), the first of a growing family of patent-pending, potentially elutable, and paramagnetic ion-exchange materials [1]. These highly selective inorganic ion-exchangers display strong chemical, thermal and radiation stability, and can be readily synthesized from low-cost materials, making them a promising alternative to organic ion-exchange resins and crystalline silicotitanate (CST). By nature, these inorganic media lend themselves more readily to volume reduction (VR) by vitrification without the issues faced with organic resins. In fact, with a simple melting of the KMS-1 media at 650–670 deg. C (i.e., well below the volatilization temperature of Cs, Sr, Mn, Fe, Sb, etc.), a VR of 4:1 was achieved. With true pyrolysis at higher temperatures or by vitrification, this VR would be much higher. The introduction of this new family of highly specific ion-exchange agents has potential to both reduce the cost of waste processing, and enable improved waste-classification management in both nuclear power plants (for the separation of Class A from B/C wastes) and DOE tank farms [for the separation of low level waste (LLW) from high level waste (HLW)]. In conclusion, we demonstrate for the first time a novel inorganic ion-exchanger for the selective removal of Cesium and Strontium. These inorganic ion-exchangers are chemical, thermal and radiation stable. These inorganic ion-exchangers can be synthesized in a cost-effective way which makes them significantly more effective than organic ion-exchange resin and CST. Finally, new thermal options are afforded for their final volume reduction, storage and disposal.

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